Theoretical studies on the impact of point defect on the structures of different uranium silicides

TL;DR

This study uses first-principles calculations to analyze how point defects and fission products affect the structure and stability of uranium silicides, providing insights into nuclear fuel behavior.

Contribution

It offers new predictions on defect stability, fission product sites, and structural changes in uranium silicides using first-principles methods.

Findings

Silicon vacancies are more common in ta-USi2.

Uranium vacancies are most stable in other structures.

Fission products prefer uranium sites, with barium causing significant volume change.

Abstract

The structures, point defects and impacts of fission products for U3Si (\b{eta}-U3Si and {\gamma}-U3Si) and USi2 ({\alpha}-USi2 and \b{eta}-USi2) are studied by first-principles calculations. The lattice parameters of U3Si and USi2 are calculated and the stability of different types of point defects is predicted by their formation energies. The results show that silicon vacancies are more prone to be produced than uranium vacancies in \b{eta}-USi2 matrix, while uranium vacancies are the most stable defects of other three types of crystallographic structures. The most favorable sites of fission products (strontium, barium, cerium and neodymium) are determined in this work as well. By calculating incorporation energies of fission products, we demonstrate that the uranium site is the most favored for all the fissions products. Comparing the structural changes influenced by different fission products, it is also found that the highest volume change is caused by barium interstitials. According to the current data, rare earth elements cerium and neodymium are found to be more stable than alkaline earth metals strontium and barium in a given nuclear matrix. Finally, it is also determined that in USi2 crystal lattice fission products tend to be stabilized in uranium substitution sites, while they are likely to form precipitates from the U3Si matrix. It is expected that this work may provide new insight into the mechanism for structural evolutions of silicide nuclear fuels in a reactor.